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1.
RSC Adv ; 14(24): 16661-16677, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38784421

RESUMO

This study explores the iodine and nickel-doped cobalt hydroxide (I & Ni-co-doped-Co(OH)2) as a potential material for energy storage and conversion applications owing to its excellent electrochemical characteristics. According to our analysis, it was revealed that this material exhibits pseudocapacitive-like behavior, as evident from distinct redox peaks observed in cyclic voltammetry, which confirms its ability to store charges. The diffusion coefficient analysis reveals that this material possesses conductivity and rapid diffusion kinetics, making it particularly advantageous compared to materials synthesized in previous studies. Charge-discharge measurements were performed to analyze the charge storage capacity and stability of this material after 3000 consecutive cycles, showing its excellent stability with minimum loss of capacitance. Furthermore, its anodic and cathodic linear sweep voltammetry curves were measured to evaluate its oxygen evolution and hydrogen evolution reaction performance. The results showed that the material exhibited an excellent water splitting performance, which suggests its potential practical application for hydrogen production. This increased activity was attributed to the doping of α-Co(OH)2, which improved its structural stability, electrical conductivity, and charge transfer efficiency. Thus, I & Ni-co-doped-Co(OH)2 possesses enhanced properties that make it an excellent material for both energy storage and hydrogen generation applications.

2.
Dalton Trans ; 53(19): 8177-8190, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38683625

RESUMO

Exploring new strategies to design non-precious and efficient electrocatalysts can provide a solution for sluggish electrocatalytic kinetics and sustainable hydrogen energy. Transition metal selenides are potential contenders for bifunctional electrocatalysis owing to their unique layered structure, low band gap, and high intrinsic activities. However, insufficient access to active sites, lethargic water dissociation, and structural degradation of active materials during electrochemical reactions limit their activities, especially in alkaline media. In this article, we report a useful strategy to assemble vanadium diselenide (VSe2) into a 3D MXene/rGO-based sponge-like architecture (VSe2@G/MXe) using hydrothermal and freeze-drying approaches. The 3D hierarchical meso/macro-pore rich sponge-like morphology not only prevents aggregation of VSe2 nanosheets but also offers a kinetics-favorable framework and high robustness to the electrocatalyst. Synergistic coupling of VSe2 and a MXene/rGO matrix yields a heterostructure with a large specific surface area, high conductivity, and multi-dimensional anisotropic pore channels for uninterrupted mass transport and gas diffusion. Consequently, VSe2@G/MXe presented superior electrochemical activity for both the HER and OER compared to its counterparts (VSe2 and VSe2@G), in alkaline media. The overpotentials required to reach a cathodic and anodic current density of 10 mA cm-2 were 153 mV (Tafel slope = 84 mV dec-1) and 241 mV (Tafel slope = 87 mV dec-1), respectively. The Rct values at the open circuit voltage were as low as 9.1 Ω and 1.41 Ω for the HER and OER activity, respectively. Importantly, VSe2@G/MXe withstands a steady current output for a long 24 h operating time. Hence, this work presents a rational design for 3D microstructures with optimum characteristics for efficient bifunctional alkaline water-splitting.

3.
RSC Adv ; 13(40): 28063-28075, 2023 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-37746331

RESUMO

Herein, nanostructured Gd-doped ZnFe2O4 (GZFO) has been synthesized via the sol-gel route and its CNT-reinforced nanohybrid was formed via an advanced ultrasonication method. The as-synthesized, hybrid electroactive materials have been supported on aluminum foil (AF) to design a flexible electrode for hybrid capacitor (HC) applications. Nanostructured material synthesis, Gd-doping, and CNT reinforcement approaches have been adopted to develop a rationally designed electrode with a high surface area, boosted electrical conductivity, and enhanced specific capacitance. Electrochemical impedance spectroscopy, galvanostatic charge/discharge, and cyclic voltammetry processes have been used to measure the electrochemical performance of the prepared ferrite material-based working electrodes in a 3M KOH solution. A nanohybrid-based working electrode (GZFO/C@AF) shows superior rate capacitive and electrochemical aptitude (specific capacitance, rate performance, and cyclic activity) than its counterpart working electrodes (ZFO@AF and GZFO@AF). The hybrid working electrode (GZFO/C@AF electrode) shows a high specific capacitance of 887 F g-1 and good retention of 94.5% for 7000 cycles (at 15 Ag-1). The maximum energy density and power density values for the GZFO/C@AF electrode are 40.025 Wh Kg-1 and 279.78 W Kg-1, respectively. Based on the findings of the electrochemical experiments, GZFO/C@AF shows promise as an electrode material for hybrid capacitors that provide energy to wearable electronic devices.

4.
RSC Adv ; 13(28): 19046-19057, 2023 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-37362336

RESUMO

Herein, we have prepared a mixed-phase Co3O4-CoFe2O4@MWCNT nanocomposite through a cheap, large-scale, and facile ultrasonication route followed by annealing. The structural, morphological, and functional group analyses of the synthesized catalysts were performed by employing various characterization approaches such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). The resultant samples were tested for bifunctional electrocatalytic activity through various electrochemical techniques: cyclic voltammetry (CV), linear sweep voltammetry (LSV), and electrochemical impedance spectroscopy (EIS). The prepared Co3O4-CoFe2O4@MWCNT nanocomposite achieved a very high current density of 100 mA cm-2 at a lower (290 mV and 342 mV) overpotential (vs. RHE) and a smaller (166 mV dec-1 and 138 mV dec-1) Tafel slope in the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively, compared to Co3O4-CoFe2O4. The excellent electrochemical activity of the as-prepared electrocatalyst was attributed to the uniform incorporation of Co3O4-CoFe2O4 over MWCNTs which provides high redox active sites, a greater surface area, better conductivity, and faster charge mobility. Furthermore, the enhanced electrochemical active surface, low charge-transfer resistance (Rct), and higher exchange current density (J0) of the Co3O4-CoFe2O4@MWCNT ternary composite are attributed to its superior behavior as a bifunctional electrocatalyst. Conclusively, this study demonstrates a novel and large-scale synthesis approach for bifunctional electrocatalysts with a high aspect ratio and abundance of active sites for high-potential energy applications.

5.
RSC Adv ; 12(36): 23454-23465, 2022 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-36090404

RESUMO

The design of oxygen evolution reaction (OER) catalysts with higher stability and activity by economical and convenient methods is considered particularly important for the energy conversion technology. Herein, a simple hydrothermal method was adopted for the synthesis of iodine-doped nickel hydroxide nanoparticles and their OER performance was explored. The electrocatalysts were structurally characterized by powder X-ray diffraction analysis (P-XRD), Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDX), and BET analysis. The electrochemical performance of the electrocatalysts was assessed by cyclic voltammetry, linear sweep voltammetry, and electrochemical impedance spectroscopy. The abundant catalytic active sites, oxygen vacancies, low charge-transfer resistance, and a high pore diameter to pore size ratio of iodine-doped Ni(OH)2 were responsible for its excellent catalytic activity, whereby OER was initiated even at 1.52 V (vs. RHE) and a 330 mV overpotential was needed to reach a 40 mV cm-2 current density in 1 M KOH solution. The material also exhibited a low Tafel slope (46 mV dec-1), which suggests faster charge-transfer kinetics as compared to its counterparts tested under the same electrochemical environment. It is worth noting that this facile and effective approach suggests a new way for the fabrication of metal hydroxides rich in oxygen vacancies, thus with the potential to boost the electrochemical performance of energy-related systems.

6.
J Hazard Mater ; 402: 123526, 2021 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-32758998

RESUMO

An efficient, environment-friendly and economical catalyst to control contaminants of environment is an enduring interest in recent years. In this study, a new composite, DyxMnFe2-xO4nanoparticles decorated over mesoporous silica was synthesized and utilized for removal of organic pollutant. Highly crystalline nature of DyxMnFe2-xO4 nanoparticles and amorphous nature of material was confirmed by XRD (X-ray diffraction) technique. Infrared spectra of fabricated material before and after adsorption of dye molecules evidenced the successful adsorption of dye molecules by fabricated adsorbent. From field emission scanning electron microscopic (FESEM) images of Dy3+ substituted MnFe2O4 composite with mesoporous silica, it was clearly observed that ferrite particles of size 20-30 nm were decorated on the surface of mesoporous silica particles and distributed well over spherical silica balls homogeneously. Its magnificent mesoporous nature was revealed from BET (nitrogen adsorption-desorption measurements) analysis. Surface area, pore volume and average pore size was found 387.95 m2/g, 0.390 cm3/g and 4.02 nm respectively. Tri-modal pore size distribution showed its effective utilization in adsorption. The abundant (SiOH) hydroxyl groups of mesoporous silica, the broad diffraction hump of silica depicted its superior loading capacity of target molecular specie inside its porous network. From band gap analysis, a red shift of 2.43 eV exhibited semiconductor photocatalysis of DyxMnFe2-xO4 nanoparticles. Degradation efficiency of bare MnFe2O4, DyxMnFe2-xO4 and mesoporous silica-based composite was tested using crystal violet dye. Its explored adsorption-photocatalysis synergy, degradation mechanism, kinetic investigation, easily recovery and remarkable recycling ability suggested that the new fabricated composite is best for environmental remediation.

7.
ACS Omega ; 5(41): 26845-26854, 2020 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-33111010

RESUMO

Recently, a new class of two-dimensional (2D) materials, called MXene, consisting of layers of transition-metal carbides and nitrides/carbonitrides has been introduced. MXene, a multifunctional material with hydrophilic nature and excellent electrical conductivity and chemical stabilities, can be applied in diverse research areas such as energy harvesting and its storage, water purification, thermal dissipation, and gas sensing. To achieve the best quality of MXene, optimization of some important synthetic parameters is highly required such as an optimized etchant concentration to remove an "A" element from the MAX phase and sonication time for the efficient exfoliation of MXene flakes. Besides, there is a need to disclose that particular solvent through which intercalation can easily be achieved. In this work, we optimized the abovementioned critical parameters for the synthesis of good-quality MXene. Our results clearly explain the variations in the quality of MXene under applied etchant concentrations, solvents for better intercalation, and optimization of sonication time for better exfoliation. The obtained results suggest that 30% HF as an etchant, dimethyl sulfoxide (DMSO) as a solvent, and 135 min as the sonication time are effective parameters for the synthesis of good-quality MXene. We expect that this report will be helpful for the young research community to synthesize good-quality MXene with the required properties.

8.
J Hazard Mater ; 394: 122593, 2020 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-32251904

RESUMO

In the current investigation, graphene (rGO)-supported cerium substituted nickel ferrite (NiCeyFe2-yO4 y = 0.05) photocatalyst was prepared via two-step wet chemical approach. The resulting NiCeyFe2-yO4/rGO nanocomposite exhibited excellent photocatalytic performance and stability. Moreover, the photocatalytic activity of NiCeyFe2-yO4/rGO nanocomposite was also investigated comparatively with NiCeyFe2-yO4 nanoparticles. As compared to the NiCeyFe2-yO4 nanoparticles, NiCeyFe2-yO4/rGO nanocomposite showed superior photocatalytic efficiency and recycling stability for MB degradation, which is two times that of bare NiCeyFe2-yO4 nanoparticles. After visible light irradiation for 70 min, 94.67 % of MB dye was removed by NiCeyFe2-yO4/rGO nanocomposite whereas only 50 % of MB dye was removed by NiCeyFe2-yO4 nanoparticles. The increase in photocatalytic performance is mainly ascribed to formation of NiCeyFe2-yO4/rGO heterojunction which not only assist in separation of photo-induced charge carriers, but also sustain a strong redox ability. Moreover, the photo-corrosion of NiCe0.05Fe1.95O4 nanoparticles is inhibited through transfer of photo-induced electrons of NiCe0.05Fe1.95O4 nanoparticles to rGO. A possible photo-degradation mechanism based on reactive species trapping experiments has been proposed. The effect of various factors like pH, temperature and catalyst dosage has also been explored. Facile synthesis method, excellent photocatalytic performance for organic pollutants and superior reusability suggest that NiCeyFe2-yO4/rGO photocatalyst possesses high potential for large-scale pollutant treatment.

9.
J Labelled Comp Radiopharm ; 60(9): 394-400, 2017 07.
Artigo em Inglês | MEDLINE | ID: mdl-28430366

RESUMO

The present study reports the syntheses of half-sandwich complexes of the type [M(η5 -C5 H4 CONH-R)(CO)3 ] (M═Re,99m Tc;R═cyclic RGD peptide (cRGDyK) for potential imaging of αv ß3 integrin expression. The 99m Tc complex was prepared directly from the reaction of [99m Tc(OH2 )3 (CO)3 ]+ with cRGDyK, doubly conjugated to Thiele's acid [(C5 H5 COOH)2 ] in water. This approach extends the viability of metal-mediated retro Diels-Alder reactions for the preparation of small molecules such as linear tripeptides to a more complex cyclic peptide carrying a [(η5 -C5 H4 )99m Tc(CO)3 ] tag. The Diels-Alder product [(C5 H5 CONH-cRGDyK)2 ] was prepared from Thiele's acid via double peptide coupling. The Re-complex [Re(η5 -C5 H4 CONH-cRGDyK)(CO)3 ] was obtained by attaching [Re(η5 -C5 H4 COOH)(CO)3 ] directly to the N-terminus of cRGDyK. The identity of the 99m Tc-complex is confirmed by chromatographic comparison with the corresponding rhenium complex, fully characterized by spectroscopic techniques.


Assuntos
Peptídeos Cíclicos/química , Compostos Radiofarmacêuticos/química , Rênio/química , Tecnécio/química , Técnicas de Química Sintética , Marcação por Isótopo , Peptídeos Cíclicos/síntese química , Compostos Radiofarmacêuticos/síntese química
10.
Phys Chem Chem Phys ; 14(30): 10732-46, 2012 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-22743649

RESUMO

Nanosized gold particles were functionalised with two types of paramagnetic surface tags, one having a nitroxide radical and the other one carrying a DTPA complex loaded with Gd(3+). Selective measurements of nitroxide-nitroxide, Gd(3+)-nitroxide and Gd(3+)-Gd(3+) distances were performed on this system and information on the distance distribution in the three types of spin pairs was obtained. A numerical analysis of the dipolar frequency distributions is presented for Gd(3+) centres with moderate magnitudes of zero-field splitting, in the range of detection frequencies and resonance fields where the high-field approximation is only roughly valid. The dipolar frequency analysis confirms the applicability of DEER for distance measurements in such complexes and gives an estimate for the magnitudes of possible systematic errors due to the non-ideality of the measurement of the dipole-dipole interaction.


Assuntos
Complexos de Coordenação/química , Gadolínio/química , Ouro/química , Nanopartículas Metálicas/química , Óxidos de Nitrogênio/química , Ácido Pentético/química , Espectroscopia de Ressonância de Spin Eletrônica , Marcadores de Spin
11.
Phys Chem Chem Phys ; 13(20): 9812-7, 2011 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-21503280

RESUMO

The factors limiting the relaxivity (r) of MRI contrast agents based on small (∼2.0 nm) gold nanoparticles functionalised with paramagnetic chelates were explored using EPR spectroscopy. The EPR analysis suggested that nanoparticle-attached chelates exhibit relatively high tumbling rates which restrict their relaxivity. Two different strategies were employed in order to test this hypothesis and hence improve the relaxivity of the nanoparticle-based contrast agents. In the first approach, the particle diameter was increased. This resulted in lower surface curvature and hence tighter ligand packing, which in turn led to increased relaxivity. In the second approach, the nanoparticles were overcoated with multilayers of oppositely charged polyelectrolytes. The restricted motion of Gd(3+) chelates coated by 2-4 polymer layers led to increased relaxivity which was dramatically reduced for thicker layers, presumably due to restricted diffusion of water molecules.


Assuntos
Meios de Contraste/química , Ouro/química , Nanopartículas Metálicas/química , Complexos de Coordenação/química , Eletrólitos/química , Espectroscopia de Ressonância de Spin Eletrônica , Gadolínio/química , Imageamento por Ressonância Magnética , Ácido Pentético/química , Polímeros/química
12.
Chem Commun (Camb) ; 46(3): 451-3, 2010 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-20066322

RESUMO

Monolayer-protected, Gd(3+)-functionalised gold nanoparticles with enhanced spin-lattice relaxivity (r(1)) were prepared; adsorption of polyelectrolytes on these materials further increased r(1) and ligand exchange with a biotin-derivatised disulfide led to a prototype avidin-targeted contrast agent.


Assuntos
Meios de Contraste/química , Gadolínio/química , Ouro/química , Imageamento por Ressonância Magnética/métodos , Nanopartículas/química , Biotina/química
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